Fluorinated chlorin chromophores for red-light-driven CO2 reduction

• Published in: Nature communications Vol. 15; no. 1; pp. 5704 - 10
• Main Authors: Yang, Shuang, Yuan, Huiqing, Guo, Kai, Wei, Zuting, Ming, Mei, Yi, Jinzhi, Jiang, Long, Han, Zhiji
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 08.07.2024; Nature Publishing Group; Nature Portfolio
• Subjects: 140/131; 140/146; 140/58; 639/638/403/934; 639/638/439/890; 639/638/77/888; Biomimetics; Carbon dioxide; Carbon dioxide concentration; Catalysis; Chromophores; Energy conversion; Fluorination; Humanities and Social Sciences; Intermediates; Irradiation; Light; Light irradiation; multidisciplinary; Noble metals; Photons; Porphyrins; Radiation; Science; Science (multidisciplinary); Solar energy; Solar energy conversion
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-024-50084-8

The utilization of low-energy photons in light-driven reactions is an effective strategy for improving the efficiency of solar energy conversion. In nature, photosynthetic organisms use chlorophylls to harvest the red portion of sunlight, which ultimately drives the reduction of CO 2 . However, a molecular system that mimics such function is extremely rare in non-noble-metal catalysis. Here we report a series of synthetic fluorinated chlorins as biomimetic chromophores for CO 2 reduction, which catalytically produces CO under both 630 nm and 730 nm light irradiation, with turnover numbers of 1790 and 510, respectively. Under appropriate conditions, the system lasts over 240 h and stays active under 1% concentration of CO 2 . Mechanistic studies reveal that chlorin and chlorinphlorin are two key intermediates in red-light-driven CO 2 reduction, while corresponding porphyrin and bacteriochlorin are much less active forms of chromophores. Using low-energy photons in light-driven reactions is an effective strategy for improving the efficiency of solar energy conversion but molecular systems that mimic such function are extremely rare in non-noble-metal catalysis. Here the authors report fluorinated chlorins as chromophores for CO 2 reduction, which catalytically produce CO under both 630 nm and 730 nm light irradiation.